StimulatedExciton–Polariton Scattering inHybrid Halide Perovskites

Halide perovskites such as methylammonium lead bromide (MAPbBr<sub>3</sub>) host tightly bound three-dimensional excitons that are robust at room temperature. The excellent optical properties of MAPbBr<sub>3</sub> allow the design of optical single-mode waveguides and cavities in the frequency range close to excitonic transitions. Taken together, these results indicate that MAPbBr<sub>3</sub> is an excellent platform for probing exciton–polariton nonlinear phenomena at room temperature. Here, we investigate the ultrafast nonequilibrium dynamics of polaritons under nonresonant femtosecond-pulsed excitation. We demonstrate the presence of a stimulated acoustic phonon-assisted scattering regime above the threshold pump fluence, characterized by the explosive growth of emission intensity, a redshift of the emission spectral maximum, spectral narrowing, and subpicosecond emission dynamics. Our theoretical findings are confirmed by experimental measurements.

Publication Details

Journal
Figshare
Published
2025-02-03
DOI
https://doi.org/10.1021/acsphotonics.4c01756.s004
Primary Topic
Strong Light-Matter Interactions
Type
article
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article

StimulatedExciton–Polariton Scattering inHybrid Halide Perovskites

Figshare
Strong Light-Matter Interactions
article

StimulatedExciton–Polariton Scattering inHybrid Halide Perovskites

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Abstract

Halide perovskites such as methylammonium lead bromide (MAPbBr<sub>3</sub>) host tightly bound three-dimensional excitons that are robust at room temperature. The excellent optical properties of MAPbBr<sub>3</sub> allow the design of optical single-mode waveguides and cavities in the frequency range close to excitonic transitions. Taken together, these results indicate that MAPbBr<sub>3</sub> is an excellent platform for probing exciton–polariton nonlinear phenomena at room temperature. Here, we investigate the ultrafast nonequilibrium dynamics of polaritons under nonresonant femtosecond-pulsed excitation. We demonstrate the presence of a stimulated acoustic phonon-assisted scattering regime above the threshold pump fluence, characterized by the explosive growth of emission intensity, a redshift of the emission spectral maximum, spectral narrowing, and subpicosecond emission dynamics. Our theoretical findings are confirmed by experimental measurements.

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Strong Light-Matter Interactions
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